On the origin of optical rotation changes during the κ-carrageenan disorder-to-order transition

dc.citation.volume333
dc.contributor.authorWestberry BP
dc.contributor.authorRio M
dc.contributor.authorWaterland MR
dc.contributor.authorWilliams MAK
dc.coverage.spatialEngland
dc.date.accessioned2024-12-02T22:22:02Z
dc.date.available2024-12-02T22:22:02Z
dc.date.issued2024-06-01
dc.description.abstractIt is well established that solutions of both polymeric and oligomeric κ-carrageenan exhibit a clear change in optical rotation (OR), in concert with gel-formation for polymeric samples, as the solution is cooled in the presence of certain ions. The canonical interpretation - that this OR change reflects a 'coil-to-helix transition' in single chains - has seemed unambiguous; the solution- or 'disordered'-state structure has ubiquitously been assumed to be a 'random coil', and the helical nature of carrageenan in the solid-state was settled in the 1970s. However, recent work has found that κ-carrageenan contains substantial helical secondary structure elements in the disordered-state, raising doubts over the validity of this interpretation. To investigate the origins of the OR, density-functional theory calculations were conducted using atomic models of κ-carrageenan oligomers. Changes were found to occur in the predicted OR owing purely to dimerization of chains, and - together with the additional effects of slight changes in conformation that occur when separated helical chains form double-helices - the predicted OR changes are qualitatively consistent with experimental results. These findings contribute to a growing body of evidence that the carrageenan 'disorder-to-order' transition is a cooperative process, and have further implications for the interpretation of OR changes demonstrated by macromolecules in general.
dc.description.confidentialfalse
dc.edition.editionJune 2024
dc.format.pagination121975-
dc.identifier.author-urlhttps://www.ncbi.nlm.nih.gov/pubmed/38494229
dc.identifier.citationWestberry BP, Rio M, Waterland MR, Williams MAK. (2024). On the origin of optical rotation changes during the κ-carrageenan disorder-to-order transition.. Carbohydr Polym. 333. (pp. 121975-).
dc.identifier.doi10.1016/j.carbpol.2024.121975
dc.identifier.eissn1879-1344
dc.identifier.elements-typejournal-article
dc.identifier.issn0144-8617
dc.identifier.number121975
dc.identifier.piiS0144-8617(24)00201-7
dc.identifier.urihttps://mro.massey.ac.nz/handle/10179/72152
dc.languageeng
dc.publisherElsevier Ltd.
dc.publisher.urihttps://www.sciencedirect.com/science/article/pii/S0144861724002017
dc.relation.isPartOfCarbohydr Polym
dc.rights(c) 2024 The Author/s
dc.rightsCC BY 4.0
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.subjectCarrageenan
dc.subjectDensity-functional theory
dc.subjectMachine learning
dc.subjectMolecular dynamics
dc.subjectOptical rotation
dc.titleOn the origin of optical rotation changes during the κ-carrageenan disorder-to-order transition
dc.typeJournal article
pubs.elements-id487547
pubs.organisational-groupOther
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